The authors gratefully acknowledge Drs. Iain McCulloch, Martin Heeney and Maxim Shkunov (Merck Chemicals, Southampton (UK)) for supplying the P3HT homopolymer and Dr. Kirill Feldman (ETH Zürich) for his expert optical microscopy contributions. This work was funded in part through a grant from the European Science Foundation through the Self-Organised Nanostructures (SONS) initiative (Project 02-PE-SONS-130 NETSOMA). DanSync is acknowledged for financial support and the BW2/HASYLAB staff for kind assistance with the X-ray diffraction experiments. H. C., S. G., C. M., C. R., and N. S. wish to express their gratitude to the proprietors and operators of Geordies' for generous in-kind contributions. Supporting Information is available online from Wiley InterScience or from the authors.